Oxidation of methane.



' UNI ED STATES PATENT OFFICE.

MAX CURT VON UN RUH, OF CHARLOTTENBURG, GERMAN Y, ASSIGNORTO SAUERSTOFF- UND STICKSTOlfF-INDUSTRIE HANSMANN & 00.,

OF VIENNA, AUSTRIA-HUNGARY, A FIRM.

OXIDATION OFQMETHANE.

No..s91,753.

German EmIpire, have invented certain new and useful nprovements in the Oxidation of Methane, of which the following is a specification.

This invention relates to an improved process of oxidizing methane by the cataliz ing action of certain contact-substances so as to form the higher oxidation-products, and separating the latter for use in the arts; and the invention consists in oxidizing methane or mixtures of gases containing a considerable amount of methane by subjecting it in presence of air or other gases containing oxygen to the action of s eci'lic vegetable prod ucts, acting as cata izing or contact-sub stances, such as bark, in such a manner that methyl alcohol'and other products of the higher oxidation of methane are formed,

stances whlch were used heretofore.

employed. Furt ermore, the

without completely burning the hydrocarand water.

It is well known that methyl alcohol and formic aldehyde are obtained by the oxidation of methane by means of gases containing oxygen in the presence of copper, pumice stone, asbestos, or mixtures 0 these substances.

In the neyt process bark of any origin, such as oak bark usedfor tannin or similar substances, such as bast, in small pieces or finely ground, are used as the catalizing or contactsubstances. These contact-substances have the advantage of acting at a considerably lower temperature than the contact-sub- Granulated copper, for instance, has been used at a temperature of. about 600 centigrade; in

the new process, however, temperatures of. from 30 to 50 centigrade are preferably used. This means a considerable economy in fuel-and a sim lification of the apparatus ontact-subw stances used in the new p ocess can easily be obtained everywhere; in many places the bark is a waste product 'of very low value and may be procured at a'very small cost.

In the new ,process natural gas is prefer-f ably used as the gas containing methane; this gas may be applied either in its natural Specification of Letters Patent. Application filed October 29, 1907. Serial No. 399,763.

, Patented June 2a, 1908.

l state, or more or less refined. By natural gas is meant a gas which is obtained from the earth in certain places, and more es ecially in the neighborhood of oil fields. his gas contains about 95-98% of methane. J After the methane has been oxidized, the higher products of oxidation, that is to say,

the mixture of methyl alcohol, formic aldehydc, and formic acid, or one or more of them,

is conducted through vessels containing caustic lime, potash or the like; or the products are conducted through a column-apparatus for the pur ose of binding the acids, such as formic LClL etc. and separatingthe oxidation-products which have different boiling points, by rectification.

Example 1. 12 liters of methaneand 36,

liters of oxygen, both well mixed and preliminarily heated up to 455 centigrade, are conducted slowly during a time of 12 hours through areaction-vessel of 4 liters capacity, filled with oak bark in pieces of about 2 to 3 mm. diameter. The product is 1,520 g. of formic aldehyde, a small quantity of methyl alcohol and some formic acid. y

Example 2. 24 liters of methane and 180 liters of air, both reliminarily heated up to 45 centigrade an well mixed, are conducted slowly during a time of 12 hours through a reactlon-vessel of 4 liters capacity, filled with oak bark in pieces of about 2 to 3 mm. diame-' ter. dehyde, a small quantity of methyl alcohol and some formic acid. The temperatures for obtaining formic aldehyde are preferably from 43 up to 46.5 centigrade. For producing more methyl alcohol and less of the other products of oxidation, a somewhat lower temperature must be used; for the production of more formic acid and less of the other products of oxidation, the temperature must be somewhat higher.

claim as new and desire to secure by Letters Patent:

1. The process: of oxidizing methane, which conslsts in subjecting methane in the presence of gases containing free oxygen to the catalizing-aetion of bark at a temperature of from 30 to 50 C.

2. The process of oxidizing methane,

The products are 1,565 g. offormic al- Having thus described my invention, I

whichl consists in subjecting natural gas in t epresence of air to the catalizing action of bark at a temperature of from 30 to 50 vC. 3. 'The process of oxidizing methane,

which consists in subjecting methane in the presence of gases containing free oxygen to he catalizing action of bark at a tempera--.

ture of from 30 to 50 C. so as to produce a mixture of'methyl alcohol, .formic aldehyde and formic acid.

4. The process of oxidizing methane, whichconsists in subjecting'natural gas in the presence of air to the catalizing action of 10 bark at a'temperature of from 30 to 50 0.,

so as to produce a mixture'of methyl alcohol,

' formic aldehyde and formic acid.

5. The process of oxidizing methane, which consists in subjecting methane in the presence of gases containing free oxygento the catalizing action'of bark at a'temperature of from 30 to 50 Cl, and then separating the formic acid or other oxidation-product from the r esulting mixture of methyl. alcohol, formic aldehyde and formic acid.

'In testimony," that I claim the foregoing'as my invention, I have signed my name in presence of two subscribing witnesses.

MAX OURT VON UNR-UH. Witnesses:

HENRY Hnsrnn, WOLDEMAR HAUPr. 

